College of Chemistry and Materials Science , Sichuan Normal University , Chengdu 610068 , Sichuan , China.
Institute of Fundamental and Frontier Sciences , University of Electronic Science and Technology of China , Chengdu 610054 , Sichuan , China.
Inorg Chem. 2019 Feb 18;58(4):2257-2260. doi: 10.1021/acs.inorgchem.8b03143. Epub 2019 Jan 28.
Electrochemical reduction is an eco-friendly alternative for energy-saving artificial N fixation. The development of this process requires efficient N reduction reaction (NRR) electrocatalysts to overcome the challenge with N activation. We show that a CrO nanoparticle-reduced graphene oxide hybrid (CrO-rGO) is as an outstanding catalyst for electrochemical N-to-NH conversion under ambient conditions. In 0.1 M HCl, CrO-rGO achieves a high NH yield of 33.3 μg h mg at -0.7 V vs RHE and a high Faradaic efficiency of 7.33% at -0.6 V vs RHE, with excellent selectivity for NH synthesis and stability. Density functional theory calculations were executed to gain further insight into the mechanisms.
电化学还原是一种节能的人工固氮替代方法。该过程的发展需要高效的氮还原反应 (NRR) 电催化剂来克服氮激活的挑战。我们表明,氧化铬纳米粒子还原氧化石墨烯杂化物 (CrO-rGO) 是一种在环境条件下电化学 N 到 NH 转化的出色催化剂。在 0.1 M HCl 中,CrO-rGO 在 -0.7 V 相对于 RHE 时实现了 33.3 μg h mg 的高 NH 产率和在 -0.6 V 相对于 RHE 时 7.33%的高法拉第效率,对 NH 合成具有优异的选择性和稳定性。执行密度泛函理论计算以进一步深入了解机制。